Themed collection PCCP Perspectives
Multimodal electrochemistry coupled microcalorimetric and X-ray probing of the capacity fade mechanisms of Nickel rich NMC – progress and outlook
Combining calorimetry with hard and soft X-ray characterization elucidates bulk and surface phenomena responsible for capacity fade in LiNi0.8Mn0.1Co0.1O2 cathodes.
Recent trends in covalent functionalization of 2D materials
Covalent functionalization of the surface is crucial in 2D materials because of their atomic thinness, large surface-to-volume ratio, and uniform surface chemical potential.
Understanding the interactions between lithium polysulfides and anchoring materials in advanced lithium–sulfur batteries using density functional theory
Computational studies based on density functional theory calculations for investigating the interactions between lithium polysulfides and anchoring materials in advanced lithium–sulfur batteries.
Significance of density functional theory (DFT) calculations for electrocatalysis of N2 and CO2 reduction reactions
Density functional theory calculations have shown great significance in improving the catalytic performance and design of CO2RR and NRR electrocatalysts in recent years.
Zooming in on the initial steps of catalytic NO reduction using metal clusters
The study of reactions relevant to heterogeneous catalysis on metal clusters with full control over the number of constituent atoms and elemental composition can lead to a detailed insight into the interactions governing catalytic functionality.
Equilibrium distribution functions: connection with microscopic dynamics
For a system at equilibrium the phase space density is time invariant. We determine what distribution, if any, is preserved by various dynamics.
Electromagnetic bioeffects: a multiscale molecular simulation perspective
We summarise methodologies, challenges and opportunities for theoretical modelling to advance current understanding of electromagnetic bioeffects for biomedicine and industry.
There is still plenty of room for layer-by-layer assembly for constructing nanoarchitectonics-based materials and devices
While the layer-by-layer (LbL) assembly method has already reached a certain maturity, there is still plenty of room for expanding its usefulness for the fabrication of nanoarchitectonics-based materials and devices.
A novel energy level detector for molecular semiconductors
Principle of energy level detection by HET. The energy of hot carriers can be controlled by the voltage VEB. When the energy surpass the barrier between base and collector (φ), hot carriers inject into the energy levels, respectively.
Multi-resolution simulation of DNA transport through large synthetic nanostructures
A new combination of coarse-grained modeling and finite element calculations enable rapid and accurate characterization of DNA transport through nanostructures of diverse geometries.
Palladium clusters, free and supported on surfaces, and their applications in hydrogen storage
Palladium clusters enhance the hydrogen storage of nanoporous carbons.
Progress towards machine learning reaction rate constants
Current status and outlook on the use and development of machine learning algorithms to predict reaction rate constants.
Photoelectron spectroscopy in molecular physical chemistry
Photoelectron spectroscopy has evolved into a powerful tool for physical chemistry and molecular physics. Some recent examples are highlighted in this perspective.
Using atomic charges to model molecular polarization
We review different models for introducing electric polarization in force fields, with special focus on methods where polarization is modelled at the atomic charge level.
Physical and chemical aspects at the interface and in the bulk of CuInSe2-based thin-film photovoltaics
Technical issues which remain in CuInSe2-based solar cells are reviewed. A study of single-crystalline Cu(In,Ga)Se2 film devices, carrier recombination analysis, and effects of alkali-metal doping and silver-alloying are particularly focused on.
Enhanced sampling without borders: on global biasing functions and how to reweight them
Global enhanced sampling techniques bias the potential energy surface of biomolecules to overcome high energy barriers. Thereby, they aim to capture extensive conformational ensembles at comparably low computational cost.
Surface modeling of photocatalytic materials for water splitting
A general understanding of the methods for the surface modeling of photocatalytic materials in recent years.
Computer-aided design of molecular machines: techniques, paradigms and difficulties
Currently, exploring the operation of a molecular machine and optimizing its performance through computational simulations seems possible, while the de novo design of an original nanoarchitecture to achieve a particular task is still very challenging.
Spectroscopic analysis focusing on ionic liquid/metal electrode and organic semiconductor interfaces in an electrochemical environment
Attenuated total reflectance ultraviolet spectroscopy can facilitate access to ionic liquid/solid substrate interfaces in an electrochemical environment.
Mechanical behaviour of inorganic solid-state batteries: can we model the ionic mobility in the electrolyte with Nernst–Einstein's relation?
The fundamental physics of Nernst–Einstein's relation assumes that the electric force is in equilibrium with the viscous force, which is not necessarily compatible with the mechanical properties of a brittle inorganic solid electrolyte.
The determination of the HOR/HER reaction mechanism from experimental kinetic data
A correct kinetic analysis of HOR/HER requires steady-state polarization curves and also account for the impact of H coverage and mass transport.
Mechanistic photophysics and photochemistry of unnatural bases and sunscreen molecules: insights from electronic structure calculations
The photophysical and photochemical mechanisms of unnatural bases and sunscreen molecules predicted by electronic structure calculations.
Polarized Raman spectroscopy in low-symmetry 2D materials: angle-resolved experiments and complex number tensor elements
Schematic of the experimental set-up to collect the angle-resolved polarized Raman spectra unveiling the optically anisotropic properties in 2D materials.
Morphological design strategies to tailor out-of-plane charge transport in conjugated polymer systems for device applications
The transport of charge carriers throughout an active conjugated polymer (CP) host, characterized by a heterogeneous morphology of locally varying degrees of order and disorder, profoundly influences the performance of CP-based electronic devices.
Computational elucidations on the role of vibrations in energy transfer processes of photosynthetic complexes
This perspective provides accounts on recent studies regarding the role of vibrations toward energy transfers in photosynthetic complexes. The latest developments in simulation techniques are also reviewed with an outlook to future directions.
Rotational action spectroscopy of trapped molecular ions
Rotational action spectroscopy is an experimental method in which rotational spectra of molecules, typically in the microwave to sub-mm-wave domain of the electromagnetic spectrum (∼1–1000 GHz), are recorded by action spectroscopy.
An overview from simple host–guest systems to progressively complex supramolecular assemblies
This perspective article presents an overall summary from simple host–guest complexation to advanced supramolecular assemblies.
Vibrational predissociation versus intramolecular vibrational energy redistribution (IVR) in rare gas⋯dihalogen complexes: IVR identified in Ar⋯I2(B, ν′) using velocity-map imaging
Contributions from competing relaxation pathways can be difficult to identify, but direct evidence for IVR in the dissociation of excited-state Ar···I2(B, v') complexes was obtained using ion product velocity map imaging.
Rechargeable aqueous zinc–bromine batteries: an overview and future perspectives
We review the past and present investigations on ZBBs, discuss the key problems and technical challenges, and propose perspectives for the future, with the focus on materials and chemistry.
On the fate of high-resolution electron energy loss spectroscopy (HREELS), a versatile probe to detect surface excitations: will the Phoenix rise again?
High-resolution electron energy loss spectroscopy is a powerful tool to investigate surface excitations (vibrations of chemisorbed atoms and molecules, phonons, plasmons). Here, a perspective on the status and the future perspectives of HREELS is presented.
Phonon transport in graphene based materials
Graphene, due to its atomic layer structure, has the highest room temperature thermal conductivity k for all known materials and many excellent thermal properties.
Laser spectroscopy of helium solvated molecules: probing the inertial response
Superfluid helium nanodroplets provide a unique environment for investigating the coupling of solvent to the rotation of embedded molecules.
Unravelling the role of charge transfer state during ultrafast intersystem crossing in compact organic chromophores
The role of the intermolecular charge transfer state during ultrafast intersystem crossing in compact chromophores is revealed by spectroscopy and theoretical investigations.
Electropumping of nanofluidic water by linear and angular momentum coupling: theoretical foundations and molecular dynamics simulations
Water confined by asymmetric hydrophobic/hydrophilic walls (left) and symmetric hydrophilic walls (right), and associated streaming velocity profiles in the steady-state after application of a rotating electric field.
The electron-transfer intermediates of the oxygen evolution reaction (OER) as polarons by in situ spectroscopy
The conversion of diffusive forms of energy (electrical and light) into short, compact chemical bonds by catalytic reactions regularly involves moving a carrier from an environment that favors delocalization to one that favors localization.
High-fidelity first principles nonadiabaticity: diabatization, analytic representation of global diabatic potential energy matrices, and quantum dynamics
This Perspective discusses recent advances in constructing high fidelity diabatic potential energy matrices for nonadiabatic systems and the associated quantum dynamics.
Strategies used by nature to fix the red, purple and blue colours in plants: a physical chemistry approach
Simple anthocyanins by themselves are unable to give significant colours in plants. In this work, the strategies used by nature to fix the flavylium cation and quinoidal base colours are investigated from the point of view of their physical chemistry.
The rise of X-ray spectroscopies for unveiling the functional mechanisms in batteries
Synchrotron-based X-ray spectroscopies have been key tools in the discovery, understanding, and development of battery materials. In this Perspective review, their state-of-the-art is highlighted, with special emphasis on future trends and needs.
Studying 2D materials with advanced Raman spectroscopy: CARS, SRS and TERS
Perspectives on advancing our understanding of two-dimensional materials using coherent anti-Stokes (CARS), stimulated (SRS) and tip-enhanced (TERS) Raman spectroscopy techniques.
Challenges in tin perovskite solar cells
Perovskite solar cells are the rising star of third-generation photovoltaic technology.
Digital-intellectual design of microporous organic polymers
In this perspective, we propose digital-intellectual materials design as the fifth stage of materials design and present its overview of microporous polymers.
Can the microscopic and macroscopic transport phenomena in deep eutectic solvents be reconciled?
A thorough understanding of the structural relaxation associated to the H-bond dynamics in DESs will provide the necessary framework to interpret the emergence of bulk transport properties from their microscopic counterparts.
Computational investigations of selected enzymes from two iron and α-ketoglutarate-dependent families
AlkB and TET are two members of the Fe and α-ketoglutarate dependent superfamily of enzymes. This perspective provides an overview of computational investigations that have been carried out to study selected members of these two families.
Solubilities in aqueous nitrate solutions that appear to reverse the law of mass action
Non-ideal aqueous electrolyte solutions have been studied since the start of the application of thermodynamics to chemistry in the late 19th century.
High-performance lithium–sulfur batteries enabled by regulating Li2S deposition
This perspective highlights the significance of regulating Li2S deposition and the related methods in improving the performance of lithium–sulfur batteries.
Understanding the molecular mechanisms of transcriptional bursting
Microscopic origins of transcriptional bursting phenomena are discussed from the physical–chemical point of view.
Solvate electrolytes for Li and Na batteries: structures, transport properties, and electrochemistry
Activity of the solvent is negligible in molten solvate electrolytes; this is the main origin of their peculiar characteristics, such as high thermal stability, wide electrochemical window, and unique ion transport.
First-principles materials simulation and design for alkali and alkaline metal ion batteries accelerated by machine learning
This Perspective is intended to reveal and envisage how the introduction of machine learning techniques accelerates first-principle materials simulation and design for alkali and alkaline metal-ion batteries.
A quantitative multiscale perspective on primary olefin formation from methanol
Our quantitative multi-scale perspective on the formation of the first C–C bond decouples the adsorption, desorption, reaction, and mobility of species and provides new insights that could guide rational catalyst design.
2D ferroelectric devices: working principles and research progress
Due to their unique reversible polarization, 2D ferroelectrics are promising for nanodevice applications in ferroelectric field effect transistors, diodes and tunnel junctions.
Structures, plasmon-enhanced luminescence, and applications of heterostructure phosphors
The structures, plasmon-enhanced luminescence and mechanism of metal/fluorophore heterostructure composites, such as core–shell nanocrystals, multilayers, adhesion, islands, arrays, and composite optical glass, are reviewed in detail.
Opportunities and challenges in microwave absorption of nickel–carbon composites
The research progress of metal magnetic Ni absorbing materials, a variety of carbon-based absorbing materials, and Ni–C composites are reviewed. The basic challenges and opportunities are prospected.
Single-layer carbon nitride: synthesis, structure, photophysical/photochemical properties, and applications
This Perspective provides a critical summary of the current state of the art in the synthesis and properties of polyheptazine single-layer carbon nitride (SLCN).
The necessity of periodic boundary conditions for the accurate calculation of crystalline terahertz spectra
Terahertz vibrational spectroscopy has emerged as a powerful spectroscopic technique, providing valuable information regarding long-range interactions – and associated collective dynamics – occurring in solids.
Breakdown of the Stokes–Einstein relation in supercooled water: the jump-diffusion perspective
The breakdown of the Stokes–Einstein relation in supercooled water can be quantitatively explained using the translational jump-diffusion approach.
Yet another perspective on hole interactions
Hole interactions are known by different names depending on their key atom (e.g. halogen, chalcogen, triel or hydrogen bonds), and the geometry of the interaction (σ, π, δ). Maybe we can make some order by analysing their molecular orbitals?
Building ordered nanoparticle assemblies inspired by atomic epitaxy
This Perspective reviews recent advances in ordered nanoparticle assemblies that are produced on selected substrates, akin to the atomic epitaxy.
Molecular modelling of compounds used for corrosion inhibition studies: a review
This perspective review features, among others, the use of DFT, QSAR modeling, artificial neural network (ANN) modeling, molecular dynamics simulations and Monte Carlo simulations in modelling organic corrosion inhibitors. It is a compendium of studies on the subject.
A perspective on the redox properties of tetrapyrrole macrocycles
Understanding the redox properties of tetrapyrroles requires deep insights into how structural/electronic alterations affect all four frontier molecular orbitals.
Single-nanoparticle spectroelectrochemistry studies enabled by localized surface plasmon resonance
Details of electrodeposition and local chemical transformations of single nanostructures can be studied using surface plasmon resonance-enabled darkfield light scattering, photoluminescence, and electrogenerated chemiluminescence.
Theoretical insights on boron reducing agent for the reduction of carbonyl compounds
We present the computational progress on boron reducing agents affecting the catalytic reductions of carbonyl compounds and discuss their future opportunities.
Kinetics of photon upconversion by triplet–triplet annihilation: a comprehensive tutorial
Kinetics of triplet–triplet annihilation photon upconversion is organized from the basics for non-experts and experts. From self-consistent analyses of the tangled photophysical events, many important and useful relations are derived and summarized.
An overview of hydroxy-based polyanionic cathode insertion materials for metal-ion batteries
Hydroxy-based polyanionic cathode materials are reviewed for (post) Li-ion batteries with a special focus on the hydroxyphosphate, hydroxysulfate and jarosite classes of insertion host materials.
Progress in phase-sensitive sum frequency generation spectroscopy
Representative methods of surface-selective phase-sensitive sum frequency generation spectroscopy are reviewed in terms of interferometer implementation for optical heterodyne detection.
Integration of theory, simulation, artificial intelligence and virtual reality: a four-pillar approach for reconciling accuracy and interpretability in computational spectroscopy
A general “four-pillar strategy” (theory, simulation, machine learning and augemented reality/virtual reality) to integrate computational and experimental spectroscopy.
Modern multireference methods and their application in transition metal chemistry
Modern multireference methods open up the possibility to treat complicated transition metal systems on a physically sound basis.
Thermal and photo stability of all inorganic lead halide perovskite nanocrystals
We shed light on the thermal and photo stability of all inorganic lead halide perovskite nanocrystals from the perspective of surface ligands and structure composition in order to promote their application from the laboratory to the market.
Label-free methods for optical in vitro characterization of protein–protein interactions
Protein–protein interactions are involved in the regulation and function of the majority of cellular processes.
The π-hole revisited
Two views of the computed electrostatic potential on the 0.001 au surface of 2,4,6-trifluoro-1,3,5-triazine. Red is the most positive color range, while blue is the most negative.
Environment-friendly Cu-based thin film solar cells: materials, devices and charge carrier dynamics
The materials, devices and charge carrier dynamics of Cu-based thin-film solar cells are comprehensively reviewed to promote the understanding of photovoltaic design.
About this collection
Welcome to our online collection of PCCP Perspective articles. Here we feature PCCP Perspective articles published in 2021.
Perspectives are high profile articles that present an authoritative state-of-the-art account of the selected research field. PCCP Perspectives take a wide variety of forms including personal accounts of research, critical analyses of topics of current interest and essential introductions to a field.
Congratulations to all the authors whose articles are featured and we hope readers enjoy this collection.